Multisite Cooperative Regulation of Solvation and Interface via Dynamic Additive Engineering for Highly Reversible...

Inexhaustible additives have been reported to enhance the reversibility of aqueous zinc-ion batteries (AZIBs). However, the structure-performance relationship of additive molecules remains elusive, particularly regarding multisite coordination-mediated synergistic regulation of solvation and interface. Herein, a dynamic configuration reconstruction mechanism that orchestrates the multisite regulation of solvation and interface is unveiled by utilizing a series of polyhydroxy additive prototypes, demonstrating that the increase of functional groups and chain flexibility in multifunctional-group molecules (MGMs) contributes to boosting battery performance. MGM with folded configuration engages in multisite Zn²⁺ coordination in the solvation shell, effectively minimizing active H₂O molecule to suppress parasitic reactions, while its configuration transition to straight-chain architecture enables multisite parallel adsorption on Zn anode interface, thus accelerating desolvation kinetics and steering (002)-facet-dominated Zn deposition. Remarkably, Zn//Zn cells achieve long cycle life of 7000 h and subzero-temperature operation, and Zn//PANI pouch cell maintains nearly 100% capacity retention after 500 cycles. This work opens a fascinating avenue for developing high-performance batteries via dynamic additive engineering.